Selective hydrogenation of 1,3-butadiene on platinum-copper alloys at the single-atom limit.

Autor: Lucci FR; Department of Chemistry, Tufts University, 62 Talbot Avenue, Medford, Massachusetts 02155, USA., Liu J; Department of Chemical and Biological Engineering, Tufts University, 4 Colby Street, Medford, Massachusetts 02155, USA., Marcinkowski MD; Department of Chemistry, Tufts University, 62 Talbot Avenue, Medford, Massachusetts 02155, USA., Yang M; Department of Chemical and Biological Engineering, Tufts University, 4 Colby Street, Medford, Massachusetts 02155, USA., Allard LF; Materials Science and Technology Division, Oak Ridge National Laboratory, PO Box 2008 MS-6064, Oak Ridge, Tennessee 37831, USA., Flytzani-Stephanopoulos M; Department of Chemical and Biological Engineering, Tufts University, 4 Colby Street, Medford, Massachusetts 02155, USA., Sykes EC; Department of Chemistry, Tufts University, 62 Talbot Avenue, Medford, Massachusetts 02155, USA.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2015 Oct 09; Vol. 6, pp. 8550. Date of Electronic Publication: 2015 Oct 09.
DOI: 10.1038/ncomms9550
Abstrakt: Platinum is ubiquitous in the production sectors of chemicals and fuels; however, its scarcity in nature and high price will limit future proliferation of platinum-catalysed reactions. One promising approach to conserve platinum involves understanding the smallest number of platinum atoms needed to catalyse a reaction, then designing catalysts with the minimal platinum ensembles. Here we design and test a new generation of platinum-copper nanoparticle catalysts for the selective hydrogenation of 1,3-butadiene,, an industrially important reaction. Isolated platinum atom geometries enable hydrogen activation and spillover but are incapable of C-C bond scission that leads to loss of selectivity and catalyst deactivation. γ-Alumina-supported single-atom alloy nanoparticle catalysts with <1 platinum atom per 100 copper atoms are found to exhibit high activity and selectivity for butadiene hydrogenation to butenes under mild conditions, demonstrating transferability from the model study to the catalytic reaction under practical conditions.
Databáze: MEDLINE